ANALYST
·
2023
·Vol. 148
·期 8
·1838-1847
·
IF 4.2
Zhidong Zhao,Yuan He,Xingrui Qi,Nian Li,Zijian He,Yufang Chen,Tao Jin
Electrochemical determination of synthetic opioids such as fentanyl is meaningful but still challenging no matter from a social or academic perspective. Herein, we report a series of novel electrocatalysts based on Fe-containing metal–organic frameworks and multi-walled carbon nanotubes (Fe-MOF/MWCNTs). The obtained Fe-MOF/MWCNT electrode materials all show ultrasensitivity on fentanyl determination. In particular, MOF-235/MWCNTs even exhibit an ultra-low limit of detection (LOD) of 0.03 μM with a wide linear range from 0.1 to 50 μM. Besides, this series of Fe-MOF/MWCNTs also displays excellent repeatability, selectivity, and stability. Moreover, they show good performance in real sample detection and achieve good recovery of 95.47%–102.41% and 96.62%–103.15% in blood and urine samples, respectively. This high performance in fentanyl determination is mainly contributed by the Fenton-like process and the adsorption function of the Fe-MOF. Therefore, these novel Fe-MOF/MWCNTs are promising electrocatalysts for point-of-care device fabrication and also have potential applications in fentanyl rapid test technology.
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LANGMUIR
·
2023
·
IF 3.9
Fengye Guo,Wenhua Li,Yefan Liu,Qianqiao Chen,Qin Zhong
Transition metal phosphides with excellent performance are one of the effective alternatives to noble metal catalysts in overall water splitting. In this paper, the Fe–NiCoP–MoO3 composite was prepared by a facile synthesis as the bifunctional electrocatalyst. Fe–NiCoP–MoO3 achieves an operating current density of 10 mA/cm2 at a low overpotential of 65 mV for hydrogen evolution reaction and drives an operating current density of 50 mA/cm2 at only 293 mV for oxygen evolution reaction. Significantly, Fe–NiCoP–MoO3 was employed as the anode and cathode for overall water splitting, which only requires a cell voltage of 1.586 V to reach 10 mA/cm2 as well as shows excellent stability. The electrocatalytic activity of Fe–NiCoP–MoO3 exceeds most of the recently reported typical bifunctional electrocatalysts. This may be due to the coupling effect between the polymetallic phosphides. In addition, heterogeneous catalysts generally expose more active sites than homogeneous catalysts. In addition, replacing MoO3 with WO3 and VO3 can also improve the performance of Fe–NiCoP. This work provides an idea for the modification of phosphides.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ruiling Sun,Guilong Yan,Xunlong Zhang,Zhenyu Li,Jingyu Chen,Li Wang,Yuanpeng Wu,Yiqun Wang,Han Li
The nanomaterials with multiple components and various heterogeneous interfaces have been considered as preferred efficient electromagnetic wave (EMW) absorbers. In this paper, Fe atoms were bonded to a zeolitic imidazole framework (Fe-ZIF) and Fe-ZIF-derived hollow porous carbon nanofibers (Fe-HPCNFs) were prepared by the microfluid electrospinning method. The EMW absorption properties of carbon nanofibers (CNFs), Fe-ZIF-derived carbon nanofibers (Fe-CNFs), and Fe-ZIF-derived hollow porous carbon nanofibers (Fe-HPCNFs) were systematically studied. The results showed that Fe-HPCNFs has the best performance, when the thickness was only 2.0 mm, the Fe-HPCNFs achieved a minimum RL loss of −46.9 dB at 17.38 GHz, with an effective absorption bandwidth of 3 GHz. The Fe-HPCNF is a flexible, ultralightweight, self-supported material as a potential high-efficiency EMW absorber.
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2023
·Vol. 29
·期 4
·293-303
·
IF 7.1
Liu Shengkun,Zhao Qiao,Han Xiaoxue,Wei Chongyang,Liang Haoting,Wang Yidan,Huang Shouying,Ma Xinbin
The interaction between a promoter and an active metal crucially impacts catalytic performance. Nowadays, the influence of promoter contents and species has been intensively considered. In this study, we investigate the effect of the iron (Fe)–zinc (Zn) proximity of Fe–Zn bimetallic catalysts on CO 2 hydrogenation performance. To eliminate the size effect, Fe 2 O 3 and ZnO nanoparticles with uniform size are first prepared by the thermal decomposition method. By changing the loading sequence or mixing method, a series of Fe–Zn bimetallic catalysts with different Fe–Zn distances are obtained. Combined with a series of characterization techniques and catalytic performances, Fe–Zn bimetallic proximity for compositions of Fe species is discussed. Furthermore, we observe that a smaller Fe–Zn distance inhibits the reduction and carburization of the Fe species and facilitates the oxidation of carbides. Appropriate proximity of Fe and Zn (i.e., Fe 1 Zn 1 -imp and Fe 1 Zn 1 -mix samples) results in a suitable ratio of the Fe 5 C 2 and Fe 3 O 4 phases, simultaneously promoting the reverse water–gas shift and Fischer–Tropsch synthesis reactions. This study provides insight into the proximity effect of bimetallic catalysts on CO 2 hydrogenation performance. Graphical Abstract
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 39
·期 10
·2685-2690
·
IF 3.146
Wu Kang,Zhang Zhongliang,Hua Fei,Ye Zhou,Li Chao,Yao Youzhi
Sewage containing antibiotics is harmful to the water environment. Here, a newly prepared iron manganese binary oxide (FMBO) activated persulfate (PDS) has excellent performance for the degradation of sulfapyridine (SPY) in an aqueous environment. The effects of initial pH, SPY, PDS concentration and FMBO dosage on the degradation ability of SPY were investigated. When the pH of FMBO/PDS was 4.0 and the initial concentration of PDS was 2.0 mmol/L, the degradation ratio of SPY could reach 94.4%. In the system of removing organic pollutants by transition metal activated PDS, SO
−• 4
and •OH radicals are generally generated, and •OH radical plays a major role. Through the identification of SPY intermediate products by LC/MS, the degradation mechanism was explored. The degradation pathway showed that the strong oxidation of FMBO and the activity of PDS promoted the production of hydroxyl radical and contributed to the degradation and transformation of antibiotics. This study shows that FMBO/PDS has high degradation efficiency in the degradation of SPY.
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Nature Sustainability
·
2022
·Vol. 6
·期 2
·169-179
·
IF 27.157
Zhang Shengbo,Han Miaomiao,Shi Tongfei,Zhang Haimin,Lin Yue,Zheng Xusheng,Zheng Li Rong,Zhou Hongjian,Chen Chun,Zhang Yunxia,Wang Guozhong,Yin Huajie,Zhao Huijun
The dominant Haber–Bosch process to produce ammonia, arguably the most important chemical in support of global food supply, is both energy and carbon intensive, resulting in substantial environmental impacts. Electrocatalytic nitrogen reduction reaction (NRR) powered by renewable electricity provides a green synthetic route for ammonia, but still suffers from insufficient yield rate and Faradaic efficiency. Single-atom electrocatalysts (SACs) have the potential to transform this catalytic process; however, controllable synthesis of SACs with high loading of active sites remains a big challenge. Here we utilize bacterial cellulose with rich oxygen functional groups to anchor iron (Fe) and cobalt (Co), realizing high density, atomically dispersed, bimetallic Fe–Co active sites. For electrocatalytic NRR, our catalyst design delivers a remarkable ammonia yield rate of 579.2 ± 27.8 μg h −1 mg cat. −1 and an exceptional Faradaic efficiency of 79.0 ± 3.8%. The combined theoretical and experimental investigations reveal that the operando change in coordination configuration from [(O-C 2 ) 3 Fe–Co(O-C 2 ) 3 ] to [(O-C 2 ) 3 Fe–Co(O-C)C 2 ] is the enabling chemistry. Our findings suggest a general approach to engineer SACs that can drive critical reactions of relevance for sustainability.
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METALLURGICAL AND MATERIALS TRANSACTIONS B-PROCESS METALLURGY AND MATERIALS PROCESSING SCIENCE
·
2022
·Vol. 53
·期 4
·2634-2646
·
IF 2.872
Huang Jingdong,Sohn Il,Kang Youngjo,Yang Xiao
Earth’s commercial and affordable zinc reserves are expected to be depleted in less than 50 years. Since electric arc furnace (EAF) dust contains a certain amount of Zn, recovery of Zn from EAF dust has become an important issue to assure a sustainable resource supply in the future. The key technical challenge is that Zn mainly occurs in EAF dust as ZnFe 2 O 4 , a very stable crystal which is difficult to reduce or leach. MgCl 2 is believed to be effective in breaking the structure of ZnFe 2 O 4 . This work investigates the fundamentals of the reaction between MgCl 2 and ZnFe 2 O 4 . Experiments show that Zn in ZnFe 2 O 4 is chlorinated to ZnCl 2 quickly with priority over Fe, implying the efficacy of MgCl 2 in separating Zn and Fe in ZnFe 2 O 4 by selective chlorination. Effects of MgCl 2 /ZnFe 2 O 4 molar ratio and temperature on the reaction are clarified. Overuse of MgCl 2 slows down the reaction and is detrimental to the selective chlorination of Zn. Temperature can effectively increase the reaction rate as well as the priority of chlorinating Zn. Utilization of MgCl 2 could be high, because evaporation of MgCl 2 is not as fast as the reaction with ZnFe 2 O 4 . According to these results, a new technology to recover Zn from EAF dust by using MgCl 2 is proposed.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Yi Liang,Peng Zhao,Jilin Zheng,Yuanyuan Chen,Yiyi Liu,Jia Zheng,Xiaogang Luo,Danqun Huo,Changjun Hou
Reasonable sensor construction for precisely real-time detecting H2O2 produced from living cells has always been of great significance and challenges. Due to the excellent catalytic efficiency and unparalleled peroxidase-like activity, single-atomic catalysts with Fe-Nx active sites show great potential in H2O2 detection. These special atomic active sites make it easier for the Fenton reaction to occur, which provides basic support for H2O2 sensors. Their application in the in situ real-time detection of H2O2 has important market prospects. Herein, single-atomic Fe catalysts with distorted graphitic carbon are obtained through a simpler preparation method. A precursor hemin@zeolitic imidazolate framework-8 (hemin@ZIF-8) is calcined at a high temperature and carbonized to get the nitrogen-carbon codoped Fe single atoms (Fe SAs-N/C) and then successfully prepare a H2O2 electrochemical sensor by modifying it on a glassy carbon electrode (GCE). Its peroxidase activity is calculated by enzymatic kinetics, which shows a better peroxidase activity compared with horseradish peroxidase and other reported single-atom (SA) materials. Moreover, the electrocatalytic kinetics is explained by Laviron calculation, which more directly confirms that it has a faster electron transfer rate. Importantly, Fe SAs-N/C@GCE has a wider linear range than sensors combined with other SA materials and a low detection limit of 0.34 μM. It is an attractive design of H2O2 sensors and single-atomic catalysts with superior substrate affinity that are novel alternatives to natural enzymes.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Minjie Xu,Xianglin Liu,Guiyao Song,Yingying Cai,Bianfang Shi,Yitao Liu,Xiaoxu Ding,Zixu Yang,Pengfei Tian,Chenxi Cao,Jing Xu
Different iron species exhibit distinct activity and selectivity in CO 2 hydrogenation reaction. Herein, by controlling calcination temperature, Fe-Al interaction in Na promoted Fe-Al catalysts has been regulated, which further leads to various compositions of iron oxide (FeO x ) and iron carbides (Fe 7 C 3 and Fe 5 C 2 ) after CO activation and CO 2 hydrogenation reaction. The phase compositions and structures of Fe-Al catalysts are carefully distinguished by multiple characterizations, including XRD, XPS, MES and TEM, and the reactivity of different phases is studied with the combination of experiments (kinetics, TP and in situ DRIFTS) and Density Functional Theory (DFT) calculations. Our FeAl350 with the highest FeC x content shows the highest CO 2 conversion of 48.2% and the lowest CO selectivity of 10.1%, and FeAl900 with the highest Fe 5 C 2 / FeC x ratio presents the highest C 5+ selectivity of 44.6%. Finally, a correlation between different compositions of iron species with the activity and selectivity of Fe-based for CO 2 hydrogenation to olefins was established.
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2022
·Vol. 103
·期 2
·505-514
·
IF 2.606
Zou Chang,Guo Xingzhong,Wang Fan,Tian Rui,Hou Yang,Liu Fu,Yang Hui
Three-dimensional macroporous heterostructural Ni-Fe hydroxides with different mole ratio (Ni x Fe (1−x) -PH) were prepared via a sol-gel process combined with phase separation, and the overall water splitting electrocatalytic activity of the resultant macroporous Ni-Fe hydroxides were investigated in detail. The as-prepared Ni-Fe hydroxide has cocontinuous skeletons and interconnected macropores with a narrow pore size distribution (~150 nm), and possesses outstanding electrocatalytic activity with an overpotential of 263 mV for oxygen evolution reaction (OER) and 175 mV for hydrogen evolution reaction (HER) at 10 mA·cm −2 in 1 M KOH, respectively. The Ni 0.6 Fe 0.4 -PH | | Ni 0.6 Fe 0.4 -PH has efficient overall water splitting performance with a cell voltage of 1.61 V at 10 mA·cm −2 and great stability. The fantastic macropore structure and strong synergistic effect between Ni-Fe hydroxides significantly reinforce the contact area between the electrocatalyst and electrolyte, and endow high electrocatalytic performance of bifunctional electrocatalysts.
The epoxide-induced sol-gel process accompanied by phase separation allows the synthesis of macroporous heterostructural Ni-Fe hydroxide bifunctional catalyst with a mass of active sites, displaying excellent electrocatalytic activity and low overpotential at several current densities for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER).
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8611-8618
·
IF 3.925
Jing Huang,Qi Shan,Yanan Fang,Ning Zhao,Xiaomiao Feng
A new simple strategy to prepare Mn–Fe Prussian blue analogue (PBA) derived oxide micromotors through co-precipitation and heat treatment is demonstrated. The morphology of the precursors could be precisely controlled from cubic-like to spherical-like by introducing citrate. Because of the synergistic catalytic reaction of bimetallic Mn–Fe oxides, micromotors with different shapes could be powered efficiently in H2O2 solution. In particular, the obtained cubic Mn–Fe oxide micromotors showed strong propulsion at a speed of 71.21 μm s−1 in 1% H2O2 solution. With dual mechanisms of adsorption bubble separation (ABS) and Fenton oxidation, the cubic Mn–Fe oxide micromotors showed extraordinary removal ability for Rhodamine B (RhB) as a simulated pollutant and could remove up to 95.2% of RhB within 30 minutes. Magnetic Fe3O4 contained in the component not only could degrade organic pollutants, but also could be recycled by magnetic field and reused with high degradation efficiency. These dual-functional metal oxide catalytic micromotors provide a practical and environmentally friendly strategy for environmental restoration.
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CATALYSIS TODAY
·
2022
·
IF 6.562
Xinyu Guo,Bo Liu,Xinhua Gao,Fugui He,Qingxiang Ma,Subing Fan,Tian-sheng Zhao,Jumei Tian,Prasert Reubroycharoen,Jianli Zhang
The hydrophilic/hydrophobic properties of catalysts greatly influence product distribution by tuning the secondary reactions during Fischer–Tropsch synthesis. Studies have confirmed that hydrophilic modification can inhibit secondary reactions. Herein, hydroxyapatite (HAP)-supported Fe catalysts (Fe/HAP) were prepared using an impregnation method. The effect of the catalyst surface properties on the product distribution in CO hydrogenation was studied. The surface hydroxyl groups on Fe/HAP promoted the growth of carbon chains and improved olefin selectivity. The addition of Na as a promoter to Fe/HAP suppressed the formation of undesirable CH 4 , further improving the selectivity for light olefins and C 5 + hydrocarbons. Compared with Fe 2 O 3 , Fe/HAP showed lower CH 4 selectivity (15%) and higher C 5 + selectivity (45%). Meanwhile, the Fe/HAP -Na catalysts with a higher selectivity of light olefins (with an O/P ratio reaching 4.51).
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